Abstract

In this paper, we report the results of abinitio calculations of photoelectron angular distributions and vibrational branching ratios for the (2+1) REMPI of H2 via the E,F1Σ+g state, and compare these with the experimental data of Anderson etal. [Chem. Phys. Lett. 105, 22 (1984)]. These results show that the observed non‐Franck–Condon behavior is predominantly due to the R dependence of the transition matrix elements, and to a lesser degree to the energy dependence. This work presents the first molecular REMPI study employing a correlated wave function to describe the Rydberg–valence mixing in the resonant intermediate state.